In 1990 Valverde left for Athletic Bilbao, eliglible for the side although he was born in Extremadura (he moved to the Basque Country still an infant). He played six seasons with the team (from 1992–94 he scored 20 goals in the league) before moving to his final club RCD Mallorca, where he was relatively used as the Balearic Islands outfit achieved top flight promotion, and retired the following summer aged 33; during his time at Athletic, he was nicknamed Txingurri (Basque for ant).

Immediately after retiring, Valverde began his career as a manager in the youth departments of former team Athletic Bilbao. Four years later he became a co-trainer in the main squad and, in 2002, he returned to head coach duties when he took over the B-side, being promoted to first-team main boss the following year; in 2003–04, the club finished fifth and qualified for the UEFA Cup.

On 28 May 2008 Valverde was appointed coach at Greek league powerhouse Olympiacos FC,[3] winning the championship in his debut campaign and addingthe cup for the double. On 8 May 2009 the club decided not to renew his contract in spite of his success, because of a financial disagreement; however, most of the players and fans were openly in favour of him staying.[4]